Magnesium-ion batteries (MIBs) have great potential in large-scale energy storage field with high capacity, excellent safety, and low cost. However, the strong solvation effect of Mg will lead to the formation of solvated ions in electrolytes with larger size and sluggish diffusion/reaction kinetics. Here, the concept of interfacial catalytic bond breaking is first introduced into the cathode design of MIBs by hybriding MoS quantum dots with VS (VS@MQDs) as the cathode. The "in situ dynamic catalysis and re-equilibration" effects can catalyze the Cl-Mg bond breaking and trigger single Mg insertion/extraction chemistries, which can significantly accelerate the diffusion and reaction kinetics, as verified by the decreased diffusion energy barriers (0.26 eV for Mg vs 2.47 eV for MgCl) and fast diffusion coefficient. Benefitting from these dynamic catalysis effects, the constructed VS@MQD-based MIBs deliver a high discharge capacity of ∼120 mA h g at 200 mA g and a long-term cyclic stability of 1000 cycles at 1 A g. The improved performance and detailed characterizations well prove that the active ions in MIBs change from MgCl/MgCl to Mg with fast kinetics.

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http://dx.doi.org/10.1021/acsami.3c03097DOI Listing

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